Solid Electrolyte Interphase Layers by Using Lithiophilic and Electrochemically Active Ionic Additives for Lithium Metal Anodes

Abstract

The use of role-assigned ionic additives with different adsorption energies and distinct electron-accepting abilities enables the construction of a multilayer solid electrolyte interphase (SEI) with a sequential structure of lithiophilic, mechanically robust, and ionpermeable layers on Li metal anodes. The uncontrollable Li dendrite formation, which is promoted by localized electric fields on the Li metal anode, is suppressed by the lithiophilic Ag-containing inner SEI and LiF + Li 3 N-enriched outer SEI with reduced overpotentials upon Li deposition.

Hexachloro-1,3-butadiene as a Functional Additive for Constructing an Efficient Solid Electrolyte Interface Layer for Long-Life Stable Li Anodes

“…The DFT calculations were conducted by using the Gaussian (G09) package to optimize and evaluate the lower unoccupied molecular orbital (LUMO)/highest occupied molecular orbital (HOMO) of all molecules under the Lee-Yang-Parr correlation functional (B3LYP) and 6-31G + G (d, p) basis set. , …”

“…Over the past several decades, researchers have made great efforts to solve the problems of dendrite Li growth and side reactions caused by the instability of the native SEI film, such as the construction of a three-dimensional (3D) current collector, the use of new solid electrolytes, − and introducing electrolyte additives. − The 3D current collector can improve the working current density up to 10 mA cm –2 by dissipating local current density via the porous structure, at the expense of loss of gravimetric/volumetric energy densities. , Solid electrolytes can prevent dendrite Li from penetrating the diaphragm mechanically to a great degree; however, they generally need to work at high temperatures (>50 °C) due to the difficulty in solid/solid interface close contact, resulting in relatively harsh actual utilization conditions. , Previous researchers indicated that it may be one of the most simple and effective methods to improve the LMBs’ performances by introducing electrolyte additives through the optimization of the compositions and morphology of the SEI layers, which will enhance their physical and chemical properties and then regulate the deposition behavior of Li + and effectively inhibit the growth of Li dendrites. , …”

“…28, 29 Previous researchers indicated that it may be one of the most simple and effective methods to improve the LMBs' performances by introducing electrolyte additives through the optimization of the compositions and morphology of the SEI layers, which will enhance their physical and chemical properties and then regulate the deposition behavior of Li + and effectively inhibit the growth of Li dendrites. 30,31 The intrinsic properties of a SEI layer mainly depend on its unique compositions and morphologies. In previous studies, LiF with high mechanical modulus is used to modify the mechanical properties of the SEI layer.…”

High energy density Na-metal batteries enabled by a tailored carbonate-based electrolyte

“…Therefore, in a distinctive and simple way, only a Li salt (LiDFBOP) was taken as the additive in F/D (1/1) according to its effect in the Li metal community. [30][31][32][33] And the introduction of LiDFBOP has a negligible effect on the ionic conductivity of the electrolyte (Fig. S3, ESI †).…”

Understanding the role of additive in the solvation structure and interfacial reactions on lithium metal anode

“…Electrolyte additives, as part of electrolyte engineering, are a promising approach to improving battery performance. There are many recent reports on lithium metal anode additives, such as tris(hexauoroisopropyl)phosphate (THFP), 31 AgNO 3 , 32 lithium disuorobis(oxalato)phosphate (LiDFBOP) [32][33][34] and LiNO 3 , 32,[35][36][37][38] CaCO 3 , 39 lithium cyano tris(2,2,2-triuoroethyl) borate (LCTFEB), 40 LiBF 4 , 41 acrylonitrile (AN), 42 tris(penta-uorophenyl)borane(TPFPB) (or tris(pentauorophenyl)phosphine; TPFPP) 43 and lithium diuoro(oxalato)borate (LiDFOB). 44 LiDFBOP is seldom reported in LSBs but LiDFBOP can reinforce the solid electrolyte interface in LSBs, 33 and shows signicant improvements in cycling performance 30 in 1,2dimethoxyethane/1,3-dioxolane (DME/DOL) electrolyte.…”